“MnFe0.5Ru0.5O3 : an above-room-temperature antiferromagnetic semiconductor”. Tan X, McCabe EE, Orlandi F, Manuel P, Batuk M, Hadermann J, Deng Z, Jin C, Nowik I, Herber R, Segre CU, Liu S, Croft M, Kang C-J, Lapidus S, Frank CE, Padmanabhan H, Gopalan V, Wu M, Li M-R, Kotliar G, Walker D, Greenblatt M, Journal of materials chemistry C : materials for optical and electronic devices 7, 509 (2019). http://doi.org/10.1039/C8TC05059G
Abstract: A transition-metal-only MnFe0.5Ru0.5O3 polycrystalline oxide was prepared by a reaction of starting materials MnO, MnO2, Fe2O3, RuO2 at 6 GPa and 1873 K for 30 minutes. A combination of X-ray and neutron powder diffraction refinements indicated that MnFe0.5Ru0.5O3 adopts the corundum (alpha-Fe2O3) structure type with space group R (3) over barc, in which all metal ions are disordered. The centrosymmetric nature of the MnFe0.5Ru0.5O3 structure is corroborated by transmission electron microscopy, lack of optical second harmonic generation, X-ray absorption near edge spectroscopy, and Mossbauer spectroscopy. X-ray absorption near edge spectroscopy of MnFe0.5Ru0.5O3 showed the oxidation states of Mn, Fe, and Ru to be 2+/3+, 3+, and similar to 4+, respectively. Resistivity measurements revealed that MnFe0.5Ru0.5O3 is a semiconductor. Magnetic measurements and magnetic structure refinements indicated that MnFe0.5Ru0.5O3 orders antiferromagnetically around 400 K, with magnetic moments slightly canted away from the c axis. Fe-57 Mossbauer confirmed the magnetic ordering and Fe3+ (S = 5/2) magnetic hyperfine splitting. First principles calculations are provided to understand the electronic structure more thoroughly. A comparison of synthesis and properties of MnFe0.5Ru0.5O3 and related corundum Mn2BB'O-6 derivatives is discussed.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.256
Times cited: 1
DOI: 10.1039/C8TC05059G
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“A general-purpose interface between fortran and the low-level functions of the ibm-pc”. Janssens K, van Espen P, Trends in analytical chemistry 7, 128 (1988). http://doi.org/10.1016/0165-9936(88)87009-2
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Chemometrics (Mitac 3)
DOI: 10.1016/0165-9936(88)87009-2
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“Electrochemical sensing of phenicol antibiotics at gold”. Pilehvar S, Dardenne F, Blust R, De Wael K, International journal of electrochemical science 7, 5000 (2012)
Abstract: Phenicols are an effective and a broad spectrum class of antibiotics which has lost favour due to their side effects on human health. A rapid and sensitive electrochemical detection system is developed for the simultaneous detection of chloramphenicol (CAP), thiamphenicol (TAP) and florfenicol (FF). The electrochemical behaviour of CAP in the presence of its derivatives was investigated by cyclic voltammetry (CV) and square wave voltammetry (SWV). At a gold electrode, CAP gives rise to a sensitive cathodic peak at −0.68V (versus SCE) in a tris buffer solution (pH 7.6). This behavior gives us the opportunity to introduce a method for sensing CAP electrochemically in the presence of its derivatives. Calibration graphs were linear in the 2.5-7.4 μmol L-1 concentration range. Deviations from linearity were observed for higher concentrations and this was interpreted to be due to kinetic limitation caused by the saturation of CAP and its reduction products onto the gold electrode surface. A limit of detection of 1 μmol L-1 was found.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.469
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“Bio-based aromatic amines from lignin-derived monomers”. Blondiaux E, Bomon J, Smolen M, Kaval N, Lemière F, Sergeyev S, Diels L, Sels B, Maes BUW, ACS Sustainable Chemistry and Engineering 7, 6906 (2019). http://doi.org/10.1021/ACSSUSCHEMENG.8B06467
Abstract: A new approach to synthesize valuable 3,4-dialkoxyanilines and alkyl propionates from lignin-derived 4-propylguaiacol and -catechol with overall isolated yields up to 65% has been described. The strategy is based on the introduction of nitrogen via a Beckmann rearrangement. Amino introduction therefore coincides with a C-defunctionalization reaction; overall a replacement of the propyl chain by an amino group is obtained. The process only requires cheap bulk chemicals as reagents/reactants and does not involve column chromatography to purify the reaction products. Furthermore, all carbon atoms from the biorenewable lignin-derived monomers are transformed into valuable compounds. Greenness was assessed by performing a Green Metrics analysis on two dialkoxyanilines. A comparison was made with literature routes for these compounds starting from a petrochemical substrate.
Keywords: A1 Journal article; Engineering sciences. Technology; Organic synthesis (ORSY); Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1021/ACSSUSCHEMENG.8B06467
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“Carbon dioxide splitting in a dielectric barrier discharge plasma : a combined experimental and computational study”. Aerts R, Somers W, Bogaerts A, Chemsuschem 8, 702 (2015). http://doi.org/10.1002/cssc.201402818
Abstract: Plasma technology is gaining increasing interest for the splitting of CO2 into CO and O2. We have performed experiments to study this process in a dielectric barrier discharge (DBD) plasma with a wide range of parameters. The frequency and dielectric material did not affect the CO2 conversion and energy efficiency, but the discharge gap can have a considerable effect. The specific energy input has the most important effect on the CO2 conversion and energy efficiency. We have also presented a plasma chemistry model for CO2 splitting, which shows reasonable agreement with the experimental conversion and energy efficiency. This model is used to elucidate the critical reactions that are mostly responsible for the CO2 conversion. Finally, we have compared our results with other CO2 splitting techniques and we identified the limitations as well as the benefits and future possibilities in terms of modifications of DBD plasmas for greenhouse gas conversion in general.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 131
DOI: 10.1002/cssc.201402818
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“Establishing uniform acceptance in force biased Monte Carlo simulations”. Neyts EC, Thijsse BJ, Mees MJ, Bal KM, Pourtois G, Journal of chemical theory and computation 8, 1865 (2012). http://doi.org/10.1021/ct2008268
Abstract: Uniform acceptance force biased Monte Carlo (UFMC) simulations have previously been shown to be a powerful tool to simulate atomic scale processes, enabling one to follow the dynamical path during the simulation. In this contribution, we present a simple proof to demonstrate that this uniform acceptance still complies with the condition of detailed balance, on the condition that the characteristic parameter lambda = 1/2 and that the maximum allowed step size is chosen to be sufficiently small. Furthermore, the relation to Metropolis Monte Carlo (MMC) is also established, and it is shown that UFMC reduces to MMC by choosing the characteristic parameter lambda = 0 [Rao, M. et al. Mol. Phys. 1979, 37, 1773]. Finally, a simple example compares the UFMC and MMC methods.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 5.245
Times cited: 20
DOI: 10.1021/ct2008268
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“Ferromagnetism and magnetoresistance in monolayered manganites Ca2-xLnxMnO4”. Maignan A, Martin C, Van Tendeloo G, Hervieu M, Raveau B, Journal of materials chemistry 8, 2411 (1998). http://doi.org/10.1039/a805393f
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 30
DOI: 10.1039/a805393f
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“High resolution electron microscopy in materials research”. Van Tendeloo G, Journal of materials chemistry 8, 797 (1998). http://doi.org/10.1039/a708240a
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 8
DOI: 10.1039/a708240a
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“Influence of internal energy and impact angle on the sticking behaviour of reactive radicals in thin a-C:H film growth: a molecular dynamics study”. Neyts E, Bogaerts A, Physical chemistry, chemical physics 8, 2066 (2006). http://doi.org/10.1039/b517563a
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.123
Times cited: 7
DOI: 10.1039/b517563a
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“The modulated structure in the melilite CA2ZnGe2O7”. van Heurck C, Van Tendeloo G, Amelinckx S, Physics and chemistry of minerals 8, 441 (1992). http://doi.org/10.1007/BF00200967
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.538
Times cited: 19
DOI: 10.1007/BF00200967
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“Selective nickel-catalyzed conversion of model and lignin-derived phenolic compounds to cyclohexanone-based polymer building blocks”. Schutyser W, Van den Bosch S, Dijkmans J, Turner S, Meledina M, Van Tendeloo G, Debecker DP, Sels BF, Chemsuschem 8, 1805 (2015). http://doi.org/10.1002/cssc.201403375
Abstract: Valorization of lignin is essential for the economics of future lignocellulosic biorefineries. Lignin is converted into novel polymer building blocks through four steps: catalytic hydroprocessing of softwood to form 4-alkylguaiacols, their conversion into 4-alkylcyclohexanols, followed by dehydrogenation to form cyclohexanones, and Baeyer-Villiger oxidation to give caprolactones. The formation of alkylated cyclohexanols is one of the most difficult steps in the series. A liquid-phase process in the presence of nickel on CeO2 or ZrO2 catalysts is demonstrated herein to give the highest cyclohexanol yields. The catalytic reaction with 4-alkylguaiacols follows two parallel pathways with comparable rates: 1) ring hydrogenation with the formation of the corresponding alkylated 2-methoxycyclohexanol, and 2) demethoxylation to form 4-alkylphenol. Although subsequent phenol to cyclohexanol conversion is fast, the rate is limited for the removal of the methoxy group from 2-methoxycyclohexanol. Overall, this last reaction is the rate-limiting step and requires a sufficient temperature (> 250 degrees C) to overcome the energy barrier. Substrate reactivity (with respect to the type of alkyl chain) and details of the catalyst properties (nickel loading and nickel particle size) on the reaction rates are reported in detail for the Ni/CeO2 catalyst. The best Ni/CeO2 catalyst reaches 4-alkylcyclohexanol yields over 80 %, is even able to convert real softwood-derived guaiacol mixtures and can be reused in subsequent experiments. A proof of principle of the projected cascade conversion of lignocellulose feedstock entirely into caprolactone is demonstrated by using Cu/ZrO2 for the dehydrogenation step to produce the resultant cyclohexanones (approximate to 80%) and tin-containing beta zeolite to form 4-alkyl-e-caprolactones in high yields, according to a Baeyer-Villiger-type oxidation with H2O2.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 71
DOI: 10.1002/cssc.201403375
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“Charge-ordering transition in iron oxide Fe4O5 involving competing dimer and trimer formation”. Ovsyannikov SV, Bykov M, Bykova E, Kozlenko DP, Tsirlin AA, Karkin AE, Shchennikov VV, Kichanov SE, Gou H, Abakumov AM, Egoavil R, Verbeeck J, McCammon C, Dyadkin V, Chernyshov D, van Smaalen S, Dubrovinsky LS, Nature chemistry 8, 501 (2016). http://doi.org/10.1038/nchem.2478
Abstract: Phase transitions that occur in materials, driven, for instance, by changes in temperature or pressure, can dramatically change the materials' properties. Discovering new types of transitions and understanding their mechanisms is important not only from a fundamental perspective, but also for practical applications. Here we investigate a recently discovered Fe4O5 that adopts an orthorhombic CaFe3O5-type crystal structure that features linear chains of Fe ions. On cooling below approximately 150 K, Fe4O5 undergoes an unusual charge-ordering transition that involves competing dimeric and trimeric ordering within the chains of Fe ions. This transition is concurrent with a significant increase in electrical resistivity. Magnetic-susceptibility measurements and neutron diffraction establish the formation of a collinear antiferromagnetic order above room temperature and a spin canting at 85 K that gives rise to spontaneous magnetization. We discuss possible mechanisms of this transition and compare it with the trimeronic charge ordering observed in magnetite below the Verwey transition temperature.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 25.87
Times cited: 51
DOI: 10.1038/nchem.2478
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“DFT Study of Synergistic Catalysis of the Water-Gas-Shift Reaction on Cu-Au Bimetallic Surfaces”. Saqlain MA, Hussain A, Siddiq DM, Leenaerts O, Leitão AA, ChemCatChem 8, 1208 (2016). http://doi.org/10.1002/cctc.201501312
Abstract: The water-gas-shift reaction (WGSR) is an important industrial process that can be significantly enhanced at suitable catalyst surfaces. In this work, we investigate the catalytic behavior of metallic Cu(1 0 0) and bimetallic Cu–Au(1 0 0) surfaces. With density functional theory calculations, the variation in the Gibbs free energy (ΔG°), the activation barriers, and the rate constants for the WGSR are calculated. The variation in ΔG° for water dissociation shows that the process is spontaneous up to 520 K on the bimetallic surface and up to 229 K on the Cu(1 0 0) surface. The calculated rate constants for the process also show that the bimetallic surface is much more reactive than the Cu(1 0 0) surface. The calculated pressure–temperature phase diagram for water dissociation shows that the partial pressure of H2O required for water dissociation on the bimetallic surface is substantially lower than that on the Cu(1 0 0) surface at all the studied temperatures. Additionally, the calculations demonstrate that the kinetics of the water-gas-shift reaction is dominated by redox processes on both the surfaces.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 4.803
Times cited: 8
DOI: 10.1002/cctc.201501312
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“Interface control by chemical and dimensional matching in an oxide heterostructure”. O'Sullivan M, Hadermann J, Dyer MS, Turner S, Alaria J, Manning TD, Abakumov AM, Claridge JB, Rosseinsky MJ, Nature chemistry 8, 347 (2016). http://doi.org/10.1038/NCHEM.2441
Abstract: Interfaces between different materials underpin both new scientific phenomena, such as the emergent behaviour at oxide interfaces, and key technologies, such as that of the transistor. Control of the interfaces between materials with the same crystal structures but different chemical compositions is possible in many materials classes, but less progress has been made for oxide materials with different crystal structures. We show that dynamical self-organization during growth can create a coherent interface between the perovskite and fluorite oxide structures, which are based on different structural motifs, if an appropriate choice of cations is made to enable this restructuring. The integration of calculation with experimental observation reveals that the interface differs from both the bulk components and identifies the chemical bonding requirements to connect distinct oxide structures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 25.87
Times cited: 28
DOI: 10.1038/NCHEM.2441
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“Atomistic simulations of graphite etching at realistic time scales”. Aussems DUB, Bal K M, Morgan TW, van de Sanden MCM, Neyts EC, Chemical science 8, 7160 (2017). http://doi.org/10.1039/C7SC02763J
Abstract: Hydrogen–graphite interactions are relevant to a wide variety of applications, ranging from astrophysics to fusion devices and nano-electronics. In order to shed light on these interactions, atomistic simulation using Molecular Dynamics (MD) has been shown to be an invaluable tool. It suffers, however, from severe timescale
limitations. In this work we apply the recently developed Collective Variable-Driven Hyperdynamics (CVHD) method to hydrogen etching of graphite for varying inter-impact times up to a realistic value of 1 ms, which corresponds to a flux of 1020 m2 s1. The results show that the erosion yield, hydrogen surface coverage and species distribution are significantly affected by the time between impacts. This can be explained by the higher probability of C–C bond breaking due to the prolonged exposure to thermal stress and the subsequent transition from ion- to thermal-induced etching. This latter regime of thermal-induced etching – chemical erosion – is here accessed for the first time using atomistic simulations. In conclusion, this study demonstrates that accounting for long time-scales significantly affects ion bombardment simulations and should not be neglected in a wide range of conditions, in contrast to what is typically assumed.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 8.668
Times cited: 3
DOI: 10.1039/C7SC02763J
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“Phosphate ion functionalization of perovskite surfaces for enhanced oxygen evolution reaction”. Yang C, Laberty-Robert C, Batuk D, Cibin G, Chadwick AV, Pimenta V, Yin W, Zhang L, Tarascon J-M, Grimaud A, The journal of physical chemistry letters 8, 3466 (2017). http://doi.org/10.1021/ACS.JPCLETT.7B01504
Abstract: Recent findings revealed that surface oxygen can participate in the oxygen evolution reaction (OER) for the most active catalysts, which eventually triggers a new mechanism for which the deprotonation of surface intermediates limits the OER activity. We propose in this work a “dual strategy” in which tuning the electronic properties of the oxide, such as La1-xSrxCoO3-delta, can be dissociated from the use of surface functionalization with phosphate ion groups (P-i) that enhances the interfacial proton transfer. Results show that the P-i functionalized La0.5Sr0.5CoO3-delta gives rise to a significant enhancement of the OER activity when compared to La0.5Sr0.5Co3-delta and LaCoO3. We further demonstrate that the P-i surface functionalization selectivity enhances the activity when the OER kinetics is limited by the proton transfer. Finally, this work suggests that tuning the catalytic activity by such a “dual approach” may be a new and largely unexplored avenue for the design of novel high-performance catalysts.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 9.353
Times cited: 31
DOI: 10.1021/ACS.JPCLETT.7B01504
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“Gel-based morphological design of zirconium metal-organic frameworks”. Bueken B, Van Velthoven N, Willhammar T, Stassin T, Stassen I, Keen DA, Baron GV, Denayer JFM, Ameloot R, Bals S, De Vos D, Bennett TD, Chemical science 8, 3939 (2017). http://doi.org/10.1039/C6SC05602D
Abstract: The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero-or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X – H, NH2, NO2, (OH)(2)), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N-2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 mm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.668
Times cited: 168
DOI: 10.1039/C6SC05602D
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“Growth mechanism of epitaxial SrTiO3 on a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface”. Spreitzer M, Klement D, Egoavil R, Verbeeck J, Kovac J, Zaloznik A, Koster G, Van Tendeloo G, Suvorov D, Rijnders G, Journal Of Materials Chemistry C 8, 518 (2020). http://doi.org/10.1039/C9TC04092G
Abstract: Sub-monolayer control over the growth at silicon-oxide interfaces is a prerequisite for epitaxial integration of complex oxides with the Si platform, enriching it with a variety of functionalities. However, the control over this integration is hindered by the intense reaction of the constituents. The most suitable buffer material for Si passivation is metallic strontium. When it is overgrown with a layer of SrTiO3 (STO) it can serve as a pseudo-substrate for the integration with functional oxides. In our study we determined a mechanism for epitaxial integration of STO with a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface using all-pulsed laser deposition (PLD) technology. A detailed analysis of the initial deposition parameters was performed, which enabled us to develop a complete protocol for integration, taking into account the peculiarities of the PLD growth, STO critical thickness, and process thermal budget, in order to kinetically trap the reaction between STO and Si and thus to minimize the thickness of the interface layer. The as-prepared oxide layer exhibits STO(001)8Si(001) out-of-plane and STO[110]8Si[100] in-plane orientation and together with recent advances in large-scale PLD tools these results represent a new technological solution for the implementation of oxide electronics on demand.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.4
Times cited: 12
DOI: 10.1039/C9TC04092G
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“Predicted Influence of Plasma Activation on Nonoxidative Coupling of Methane on Transition Metal Catalysts”. Engelmann Y, Mehta P, Neyts EC, Schneider WF, Bogaerts A, Acs Sustainable Chemistry &, Engineering 8, 6043 (2020). http://doi.org/10.1021/acssuschemeng.0c00906
Abstract: The combination of catalysis and nonthermal plasma holds promise for enabling difficult chemical conversions. The possible synergy between both depends strongly on the nature of the reactive plasma species and the catalyst material. In this paper, we show how vibrationally excited species and plasma-generated radicals interact with transition metal catalysts and how changing the catalyst material can improve the conversion rates and product selectivity. We developed a microkinetic model to investigate the impact of vibrational excitations and plasma-generated radicals on the nonoxidative coupling of methane over transition metal surfaces. We predict a significant increase in ethylene formation for vibrationally excited methane. Plasma-generated radicals have a stronger impact on the turnover frequencies with high selectivity toward ethylene on noble catalysts and mixed selectivity on non-noble catalysts. In general, we show how the optimal catalyst material depends on the desired products as well as the plasma conditions.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
Impact Factor: 8.4
DOI: 10.1021/acssuschemeng.0c00906
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“Plasma-Based N2Fixation into NOx: Insights from Modeling toward Optimum Yields and Energy Costs in a Gliding Arc Plasmatron”. Vervloessem E, Aghaei M, Jardali F, Hafezkhiabani N, Bogaerts A, Acs Sustainable Chemistry &, Engineering 8, 9711 (2020). http://doi.org/10.1021/acssuschemeng.0c01815
Abstract: Plasma technology provides a sustainable, fossil-free method for N2 fixation, i.e., the conversion of inert atmospheric N2 into valuable substances, such as NOx or ammonia. In this work, we present a novel gliding arc plasmatron at atmospheric pressure for NOx production at different N2/O2 gas feed ratios, offering a promising NOx yield of 1.5% with an energy cost of 3.6 MJ/mol NOx produced. To explain the underlying mechanisms, we present a chemical kinetics model, validated by experiments, which provides insight into the NOx formation pathways and into the ambivalent role of the vibrational kinetics. This allows us to pinpoint the factors limiting the yield and energy cost, which can help to further improve the process.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 8.4
DOI: 10.1021/acssuschemeng.0c01815
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“Boosting biomolecular interactions through DNA origami nano-tailored biosensing interfaces”. Rutten I, Daems D, Lammertyn J, Journal Of Materials Chemistry B 8, 3606 (2020). http://doi.org/10.1039/C9TB02439E
Abstract: The interaction between a bioreceptor and its target is key in developing sensitive, specific and robust diagnostic devices. Suboptimal interbioreceptor distances and bioreceptor orientation on the sensor surface, resulting from uncontrolled deposition, impede biomolecular interactions and lead to a decreased biosensor performance. In this work, we studied and implemented a 3D DNA origami design, for the first time comprised of assay specifically tailored anchoring points for the nanostructuring of the bioreceptor layer on the surface of disc-shaped microparticles in the continuous microfluidic environment of the innovative EvalutionTM platform. This bioreceptor immobilization strategy resulted in the formation of a less densely packed surface with reduced steric hindrance and favoured upward orientation. This increased bioreceptor accessibility led to a 4-fold enhanced binding kinetics and a 6-fold increase in binding efficiency compared to a directly immobilized non-DNA origami reference system. Moreover, the DNA origami nanotailored biosensing concept outperformed traditional aptamer coupling with respect to limit of detection (11 × improved) and signal-to-noise ratio (2.5 × improved) in an aptamer-based sandwich bioassay. In conclusion, our results highlight the potential of these DNA origami nanotailored surfaces to improve biomolecular interactions at the sensing surface, thereby increasing the overall performance of biosensing devices. The combination of the intrinsic advantages of DNA origami together with a smart design enables bottom-up nanoscale engineering of the sensor surface, leading towards the next generation of improved diagnostic sensing devices.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 7
Times cited: 2
DOI: 10.1039/C9TB02439E
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“Engineering Au/MnO₂, hierarchical nanoarchitectures for ethanol electrochemical valorization”. Bigiani L, Andreu T, Maccato C, Fois E, Gasparotto A, Sada C, Tabacchi G, Krishnan D, Verbeeck J, Ramon Morante J, Barreca D, Journal Of Materials Chemistry A 8, 16902 (2020). http://doi.org/10.1039/D0TA05972B
Abstract: The design of eco-friendly electrocatalysts for ethanol valorization is an open challenge towards sustainable hydrogen production. Herein we present an original fabrication route to effective electrocatalysts for the ethanol oxidation reaction (EOR). In particular, hierarchical MnO(2)nanostructures are grown on high-area nickel foam scaffolds by a plasma-assisted strategy and functionalized with low amounts of optimally dispersed Au nanoparticles. This strategy leads to catalysts with a unique morphology, designed to enhance reactant-surface contacts and maximize active site utilization. The developed nanoarchitectures show superior performances for ethanol oxidation in alkaline media. We reveal that Au decoration boosts MnO(2)catalytic activity by inducing pre-dissociation and pre-oxidation of the adsorbed ethanol molecules. This evidence validates our strategy as an effective route for the development of green electrocatalysts for efficient electrical-to-chemical energy conversion.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 11.9
Times cited: 16
DOI: 10.1039/D0TA05972B
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“Graphene hetero-multilayer on layered platinum mineral Jacutingaite (Pt₂HgSe₃): Van der Waals heterostructures with novel optoelectronic and thermoelectric performances”. Bafekry A, Obeid M, Nguyen C, Bagheri Tagani M, Ghergherehchi M, Journal Of Materials Chemistry A 8, 13248 (2020). http://doi.org/10.1039/D0TA02847A
Abstract: Motivated by the recent successful synthesis of the layered platinum mineral jacutingaite (Pt2HgSe3), we have studied the optoelectronic, mechanical, and thermoelectric properties of graphene hetero-multilayer on Pt(2)HgSe(3)monolayer (PHS) heterostructures (LG/PHS) by using first-principles calculations. PHS is a topological insulator with a band gap of about 160 meV with fully relativistic calculations; when graphene layers are stacked on PHS, a narrow band gap of similar to 10-15 meV opens. In the presence of gate-voltage and out-of plane strain,i.e.pressure, the electronic properties are modified; the Dirac-cone of graphene can be shifted upwards (downward) to a lower (higher) binding energy. The absorption spectrum shows two peaks, which are located around 216 nm (5.74 eV) and protracted to 490 nm (2.53 eV), indicating that PHS could absorb more visible light. Increasing the number of graphene layers on PHS has a positive impact on the UV-vis light absorption and gives a clear red-shift with enhanced absorption intensity. To investigate the electronic performance of the heterostructure, the electrical conductance and thermopower of a device composed of graphene layers and PHS is examined by a combination of DFT and Green function formalism. The number of graphene layers can significantly tune the thermopower and electrical conductance. This analysis reveals that the heterostructures not only significantly affect the electronic properties, but they can also be used as an efficient way to modulate the optic and thermoelectric properties.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 11.9
Times cited: 20
DOI: 10.1039/D0TA02847A
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“Nitrogen fixation with water vapor by nonequilibrium plasma : toward sustainable ammonia production”. Gorbanev Y, Vervloessem E, Nikiforov A, Bogaerts A, Acs Sustainable Chemistry &, Engineering 8, 2996 (2020). http://doi.org/10.1021/ACSSUSCHEMENG.9B07849
Abstract: Ammonia is a crucial nutrient used for plant growth and as a building block in the pharmaceutical and chemical industry, produced via nitrogen fixation of the ubiquitous atmospheric N2. Current industrial ammonia production relies heavily on fossil resources, but a lot of work is put into developing nonfossil-based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as a H source for nitrogen fixation into NH3 by nonequilibrium plasma. The highest selectivity toward NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor contents. We also studied the role of H2O vapor and of the plasma-exposed liquid H2O in nitrogen fixation by using isotopically labeled water to distinguish between these two sources of H2O. We show that added H2O vapor, and not liquid H2O, is the main source of H for NH3 generation. The studied catalyst- and H2-free method offers excellent selectivity toward NH3 (up to 96%), with energy consumption (ca. 95–118 MJ/mol) in the range of many plasma-catalytic H2-utilizing processes.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 8.4
Times cited: 14
DOI: 10.1021/ACSSUSCHEMENG.9B07849
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“Origin of the extra capacity in nitrogen-doped porous carbon nanofibers for high-performance potassium ion batteries”. Liu F, Meng J, Xia F, Liu Z, Peng H, Sun C, Xu L, Van Tendeloo G, Mai L, Wu J, Journal Of Materials Chemistry A 8, 18079 (2020). http://doi.org/10.1039/D0TA05626J
Abstract: While graphite has limited capacity as an anode material for potassium-ion batteries, nitrogen-doped carbon materials are more promising as extra capacity can usually be produced. However, the mechanism behind the origin of the extra capacity remains largely unclear. Here, the potassium storage mechanisms have been systematically studied in freestanding and porous N-doped carbon nanofibers with an additional similar to 100 mA h g(-1)discharge capacity at 0.1 A g(-1). The extra capacity is generated in the whole voltage window range from 0.01 to 2 V, which corresponds to both surface/interface K-ion absorptions due to the pyridinic N and pyrrolic N induced atomic vacancies and layer-by-layer intercalation due to the effects of graphitic N. As revealed by transmission electron microscopy, the N-doped samples have a clear and enhanced K-intercalation reaction. Theoretical calculations confirmed that the micropores with pyridinic N and pyrrolic N provide extra sites to form bonds with K, resulting in the extra capacity at high voltage. The chemical absorption of K-ions occurring inside the defective graphitic layer will prompt fast diffusion of K-ions and full realization of the intercalation capacity at low voltage. The approach of preparing N-doped carbon-based materials and the mechanism revealed by this work provide directions for the development of advanced materials for efficient energy storage.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 11.9
Times cited: 2
DOI: 10.1039/D0TA05626J
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“Producing oxygen and fertilizer with the Martian atmosphere by using microwave plasma”. Kelly S, Verheyen C, Cowley A, Bogaerts A, Chem 8, 2797 (2022). http://doi.org/10.1016/j.chempr.2022.07.015
Abstract: We explorethepotentialofmicrowave(MW)-plasma-based in situ
utilizationoftheMartianatmospherewithafocusonthenovelpos-
sibilityoffixingN2 forfertilizerproduction. Conversioninasimulant
plasma (i.e., 96% CO2, 2% N2, and 2% Ar),performedunderen-
ergyconditionssimilartothoseoftheMarsOxygen In Situ Resource
UtilizationExperiment(MOXIE),currentlyonboardNASA’sPerse-
verancerover,demonstratesthatO/O2 formedthroughCO2 dissociation
facilitatesthefixationoftheN2 fractionviaoxidationtoNOx.
PromisingproductionratesforO2, CO,andNOx of 47.0,76.1,and
1.25g/h,respectively,arerecordedwithcorrespondingenergy
costs of0.021,0.013,and0.79kWh/g,respectively.Notably,O2
productionratesare 30 timeshigherthanthosedemonstrated
by MOXIE,whiletheNOx production raterepresentsan 7% fixa-
tionoftheN2 fraction presentintheMartian atmosphere.MW-
plasma-basedconversionthereforeshowsgreatpotentialasan in
situ resourceutilization(ISRU)technologyonMarsinthatitsimulta-
neouslyfixesN2 and producesO2.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 23.5
DOI: 10.1016/j.chempr.2022.07.015
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“Electrocatalytic oxidation of water by OH- –, and H₂O-capped IrOx nanoparticles electrophoretically deposited on graphite and basal plane HOPG : effect of the substrate electrode”. Mirbagheri N, Campos R, Ferapontova EE, Chemelectrochem 8, 1632 (2021). http://doi.org/10.1002/CELC.202100317
Abstract: Iridium oxide (IrOx) is one of the most efficient electrocatalysts for water oxidation reaction (WOR). Here, WOR electrocatalysis by 1.6 nm IrOx nanoparticles (NPs) electrophoretically deposited onto spectroscopic graphite (Gr) and basal plane highly ordered pyrolytic graphite (HOPG) was studied as a function of NPs' capping ligands and electrodeposition substrate. On Gr, OH-- and H2O-capped NPs exhibited close sub-monolayer surface coverages and specific electrocatalytic activity of 18.9-23.5 mA nmol(-1) of Ir-IV/V sites, at 1 V and pH 7. On HOPG, OH--capped NPs produced films with a diminished WOR activity of 5.17 +/- 2.40 mA nmol(-1). Electro-wettability-induced changes impeded electrophoretic deposition of H2O-capped NPs on HOPG, WOR currents being 25-fold lower than observed for OH--capped ones. The electrocatalysis efficiency correlated with hydrophilic properties of the substrate electrodes, affecting morphological and as a result catalytic properties of the formed IrOx films. These results, important both for studied and related carbon nanomaterials systems, allow fine-tuning of electrocatalysis by a proper choice of the substrate electrode.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 4.136
DOI: 10.1002/CELC.202100317
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“Elemental concentrations in aerosols at the Belgian coast versus seasons and air mass trajectories”. van Meel K, Horemans B, Krata A, Bencs L, Buczyńska AJ, Dirtu AC, Worobiec A, Van Grieken R, Environmental chemistry letters 8, 157 (2010). http://doi.org/10.1007/S10311-009-0203-4
Abstract: Marine aerosols have extensively been monitored in the framework of a research project to investigate the inorganic and organic nutrient fluxes of the atmospheric nitrogen input into the North Sea. As a part of this project bulk analysis was also performed by energy dispersive X-ray fluorescence (EDXRF) on a total of 366 samples in order to provide detailed elemental composition. Samples have been clustered per campaign and differences were related to backward trajectories. Elements as Cl, Si, and S appeared to be the best tracers for coastal aerosols. Therefore they have been chosen to represent each campaign and to map the seasonal variations. It is clear that Cl is an excellent tracer for oceanic trajectories, while a less clear correlation between the soil dust components and the air mass trajectories is found.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Laboratory Experimental Medicine and Pediatrics (LEMP); Toxicological Centre
DOI: 10.1007/S10311-009-0203-4
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“High-throughput computational screening of 2D materials for thermoelectrics”. Sarikurt S, Kocabas T, Sevik C, Journal Of Materials Chemistry A 8, 19674 (2020). http://doi.org/10.1039/D0TA04945J
Abstract: High-performance thermoelectric materials are critical in recuperating the thermal losses in various machinery and promising in renewable energy applications. In this respect, the search for novel thermoelectric materials has attracted considerable attention. In particular, low dimensional materials have been proposed as potential candidates due to their unique and controllable thermal and electronic transport properties. The considerable potential of several two-dimensional materials as thermoelectric devices has already been uncovered and many new candidates that merit further research have been suggested. In this regard, we comprehensively investigate the thermoelectric coefficients and electronic fitness function (EFF) of a large family of structurally isotropic and anisotropic two-dimensional layered materials using density functional theory combined with semi-classical Boltzmann transport theory. With this high-throughput screening, we bring to light additional 2D crystals that haven't been previously classified as favorable TE materials. We predict that Pb2Se2, GeS2, As-2, NiS2, Hf2O6, Zr2O6, AsBrS, ISbTe, ISbSe, AsISe, and AsITe are promising isotropic thermoelectric materials due to their considerably high EFF values. In addition to these materials, Hf2Br4, Zr2Br4, Hf2Cl4, Zr2Cl4, Hf2O6, Zr(2)O(6)and Os(2)O(4)exhibit strong anisotropy and possess prominently high EFF values.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 11.9
DOI: 10.1039/D0TA04945J
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“Tackling the problem of sensing commonly abused drugs through nanomaterials and (bio)recognition approaches”. Truta F, Florea A, Cernat A, Tertis M, Hosu O, De Wael K, Cristea C, Frontiers In Chemistry 8, 561638 (2020). http://doi.org/10.3389/FCHEM.2020.561638
Abstract: We summarize herein the literature in the last decade, involving the use of nanomaterials and various (bio)recognition elements, such as antibodies, aptamers and molecularly imprinted polymers, for the development of sensitive and selective (bio)sensors for illicit drugs with a focus on electrochemical transduction systems. The use and abuse of illicit drugs remains an increasing challenge for worldwide authorities and, therefore, it is important to have accurate methods to detect them in seized samples, biological fluids and wastewaters. They are recently classified as the latest group of “emerging pollutants,” as their consumption has increased tremendously in recent years. Nanomaterials, antibodies, aptamers and molecularly imprinted polymers have gained much attention over the last decade in the development of (bio)sensors for a myriad of applications. The applicability of these (nano)materials, functionalized or not, has significantly increased, and are therefore highly suitable for use in the detection of drugs. Lately, such functionalized nanoscale materials have assisted in the detection of illicit drugs fingerprints, providing large surface area, functional groups and unique properties that facilitate sensitive and selective sensing. The review discusses the types of commonly abused drugs and their toxicological implications, classification of functionalized nanomaterials (graphene, carbon nanotubes), their fabrication, and their application on real samples in different fields of forensic science. Biosensors for drugs of abuse from the last decade's literature are then exemplified. It also offers insights into the prospects and challenges of bringing the functionalized nanobased technology to the end user in the laboratories or in-field.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 5.5
DOI: 10.3389/FCHEM.2020.561638
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